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Pushing and Pulling on OH-and H3O+ with Electric Fields Across Water’s Surface

preprint
submitted on 01.04.2021, 01:23 and posted on 01.04.2021, 13:17 by kamal ray, Aditya Limaye, Ankur Saha, Ka Chon Ng, Adam Willard, Heather Allen

We use second harmonic generation spectroscopy, molecular dynamics simulation, and theoretical modeling to study the response of the neat liquid water-air interface to changes in the potential of an external electrode positioned above the liquid. We observe a parabolic dependence of second harmonic intensity on applied potential, indicating that water’s net interfacial dipole responds linearly. We also observe a minimum intensity when the potential is tuned to a specific positive value. Interpreting this minimum based on the macroscopic electrostatic potential profile yields misleading physical conclusions because it neglects the internal bias exerted on molecular orientations by the excess surface concentrations of OH- or H3O+. We thus find that water’s net interfacial dipole orientation is primarily responsive to the effects of these ionic species rather than the external electric field.

Funding

“This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under Awards # DE-SC0016381 and # DE-SC0018094, Allen and Willard Labs, respectively.

History

Email Address of Submitting Author

ray.727@osu.edu

Institution

Ohio State University

Country

USA

ORCID For Submitting Author

0000-0002-9764-7147

Declaration of Conflict of Interest

The authors declare no competing interests.

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